In hybrid metal halide perovskites, chiroptical properties typically arise from structural symmetry breaking by incorporating a chiral A-site organic cation within the structure, which may limit the compositional space. Here we demonstrate highly efficient remote chirality transfer where chirality is imposed on an otherwise achiral hybrid metal halide semiconductor by a proximal chiral molecule that is not interspersed as part of the structure yet leads to large circular dichroism dissymmetry factors (g) of up to 10. Density functional theory calculations reveal that the transfer of stereochemical information from the chiral proximal molecule to the inorganic framework is mediated by selective interaction with divalent metal cations.
View Article and Find Full Text PDFTwo-dimensional (2D) hybrid organic/inorganic perovskites are an emerging materials class for optoelectronic and spintronic applications due to strong excitonic absorption and emission, large spin-orbit coupling, and Rashba spin-splitting effects. For many of the envisioned applications, tuning the majority charge carrier (electron or hole) concentration is desirable, but electronic doping of metal-halide perovskites has proven to be challenging. Here, we demonstrate electron injection into the lower-energy branch of the Rashba-split conduction band of 2D phenethylammonium lead iodide by means of n-type molecular doping at room temperature.
View Article and Find Full Text PDFSpin accumulation in semiconductor structures at room temperature and without magnetic fields is key to enable a broader range of optoelectronic functionality. Current efforts are limited owing to inherent inefficiencies associated with spin injection across semiconductor interfaces. Here we demonstrate spin injection across chiral halide perovskite/III-V interfaces achieving spin accumulation in a standard semiconductor III-V (AlGa)InP multiple quantum well light-emitting diode.
View Article and Find Full Text PDFACS Appl Mater Interfaces
June 2024
We present time-resolved Kerr rotation (TRKR) spectra in thin films of CHNHPbI (MAPI) hybrid perovskite using a unique picosecond microscopy technique at 4 K having a spatial resolution of 2 μm and temporal resolution of 1 ps, subjected to both an in-plane applied magnetic field up to 700 mT and an electric field up to 10 V/cm. We demonstrate that the obtained TRKR dynamics and spectra are substantially inhomogeneous across the MAPI films with prominent resonances at the exciton energy and interband transition of this compound. From the obtained quantum beating response as a function of magnetic field in the Voigt configuration, we also extract the inhomogeneity of the electron and hole Lande -values and spin coherence time, *.
View Article and Find Full Text PDFTwo-dimensional (2D) hybrid organic-inorganic perovskites (HOIPs) with enhanced stability, high tunability, and strong spin-orbit coupling have shown great potential in vast applications. Here, we extend the already rich functionality of 2D HOIPs to a new territory, realizing topological superconductivity and Majorana modes for fault-tolerant quantum computation. Especially, we predict that room-temperature ferroelectric BAPbCl (BA for benzylammonium) exhibits topological nodal-point superconductivity (NSC) and gapless Majorana modes on selected edges and ferroelectric domain walls when proximity-coupled to an s-wave superconductor and an in-plane Zeeman field, attractive for experimental verification and application.
View Article and Find Full Text PDFChiral materials exhibit many interesting physical properties including circular dichroism, circularly polarized photoluminescence, and spin selectivity. Since its discovery, chirality-induced spin selectivity (CISS) has been demonstrated in many chiral material systems, which indicates promising applications in spintronic devices. Thus, searching for compounds that possess both sizable chirality and excellent spin transport properties is in order.
View Article and Find Full Text PDFThe relationship between the structural asymmetry and optoelectronic properties of functional materials is an active area of research. The movement of charges through an oriented chiral medium depends on the spin configuration of the charges, and such systems can be used to control spin populations without magnetic components - termed the chiral-induced spin selectivity (CISS) effect. CISS has mainly been studied in chiral organic molecules and their assemblies.
View Article and Find Full Text PDFACS Appl Mater Interfaces
February 2023
Understanding the stability and degradation of organic light-emitting diodes (OLEDs) under working conditions is a significant area of research for developing more effective OLEDs and further improving their performance. However, studies of degradation processes by in situ noninvasive methods have not been adequately developed. In this work, tris-(8-hydroxyquinolino) aluminum (Alq)-based OLED degradation processes have been analyzed through the investigation of the device dispersive magneto-electroluminescence (MEL()) response measured at room temperature.
View Article and Find Full Text PDFUtilizing the spin degree of freedom of photoexcitations in hybrid organic inorganic perovskites for quantum information science applications has been recently proposed and explored. However, it is still unclear whether the stable photoexcitations in these compounds correspond to excitons, free/trapped electron-hole pairs, or charged exciton complexes such as trions. Here we investigate quantum beating oscillations in the picosecond time-resolved circularly polarized photoinduced reflection of single crystal methyl-ammonium tri-iodine perovskite (MAPbI) measured at cryogenic temperatures.
View Article and Find Full Text PDFThe Rashba splitting in hybrid organic-inorganic lead-halide perovskites (HOIP) is particularly promising and yet controversial, due to questions surrounding the presence or absence of inversion symmetry. Here we utilize two-photon absorption spectroscopy to study inversion symmetry breaking in different phases of these materials. This is an all-optical technique to observe and quantify the Rashba effect as it probes the bulk of the materials.
View Article and Find Full Text PDFHigh- molecular magnets have amassed much promise; however, the long-standing obstacle for its practical applications is the inaccessibility of high-temperature molecular magnets showing dynamic and nonvolatile magnetization control. In addition, its functional durability is prone to degradation in oxygen and heat. Here, we introduce a rapid prototyping and stabilizing strategy for high (360 K) molecular magnets with precise spatial control in geometry.
View Article and Find Full Text PDFThe convergence of proton conduction and multiferroics is generating a compelling opportunity to achieve strong magnetoelectric coupling and magneto-ionics, offering a versatile platform to realize molecular magnetoelectrics. Here we describe machine learning coupled with additive manufacturing to accelerate the design strategy for hydrogen-bonded multiferroic macromolecules accompanied by strong proton dependence of magnetic properties. The proton switching magnetoelectricity occurs in three-dimensional molecular heterogeneous solids.
View Article and Find Full Text PDFIn traditional optoelectronic approaches, control over spin, charge, and light requires the use of both electrical and magnetic fields. In a spin-polarized light-emitting diode (spin-LED), charges are injected, and circularly polarized light is emitted from spin-polarized carrier pairs. Typically, the injection of carriers occurs with the application of an electric field, whereas spin polarization can be achieved using an applied magnetic field or polarized ferromagnetic contacts.
View Article and Find Full Text PDFHybrid organic-inorganic metal-halide perovskites have emerged as versatile materials for enabling low-cost, mechanically flexible optoelectronic applications. The progress has been commendable; however, technological breakthroughs have outgrown the basic understanding of processes occurring in bulk and at device interfaces. Here, we investigated the photocurrent at perovskite/organic semiconductor interfaces in relation to the microstructure of electronically active layers.
View Article and Find Full Text PDFTwo-dimensional hybrid organic-inorganic perovskites (2D-HOIPs) that form natural multiple quantum wells have attracted increased research interest due to their interesting physics and potential applications in optoelectronic devices. Recent studies have shown that spintronics applications can also be introduced to 2D-HOIPs upon integrating chiral organic ligands into the organic layers. Here we report spin-dependent photovoltaic and photogalvanic responses of optoelectronic devices based on chiral 2D-HOIPs, namely, (-MBA)PbI and (-MBA)PbI.
View Article and Find Full Text PDFSolution-processable two-dimensional (2D) organic-inorganic hybrid perovskite (OIHP) quantum wells naturally self-assemble through weak van der Waals forces. In this study, we investigate the structural and optoelectronic properties of 2D-layered butylammonium (CHNH, BA) methylammonium (CHNH, MA) lead iodide, (BA)(MA)PbI quantum wells with varying from 1 to 4. Through conventional structural characterization, (BA)(MA)PbI thin films showcase high-quality phase () purity.
View Article and Find Full Text PDFThe isotope effect is studied in the magneto-electroluminescence (MEL) and pulsed electrically detected magnetic resonance of organic light-emitting diodes based on thermally activated delayed fluorescence (TADF) from donor-acceptor exciplexes that are either protonated (H) or deuterated (D). It is found that at ambient temperature, the exchange of H to D has no effect on the spin-dependent current and MEL responses in the devices. However, at cryogenic temperatures, where the reverse intersystem crossing (RISC) from triplet to singlet exciplex diminishes, a pronounced isotope effect is observed.
View Article and Find Full Text PDFSpin waves, quantized as magnons, have low energy loss and magnetic damping, which are critical for devices based on spin-wave propagation needed for information processing devices. The organic-based magnet [V(TCNE) ; TCNE = tetracyanoethylene; x ≈ 2] has shown an extremely low magnetic damping comparable to, for example, yttrium iron garnet (YIG). The excitation, detection, and utilization of coherent and non-coherent spin waves on various modes in V(TCNE) is demonstrated and show that the angular momentum carried by microwave-excited coherent spin waves in a V(TCNE) film can be transferred into an adjacent Pt layer via spin pumping and detected using the inverse spin Hall effect.
View Article and Find Full Text PDFWe have experimentally tested whether spin-transport and charge-transport in pristine π-conjugated polymer films at room temperature occur via the same electronic processes. We have obtained the spin diffusion coefficient of several π-conjugated polymer films from the spin diffusion length measured by the technique of inverse spin Hall effect and the spin relaxation time measured by pulsed electrically detected magnetic resonance spectroscopy. The charge diffusion coefficient was obtained from the time-of-flight mobility measurements on the same films.
View Article and Find Full Text PDFWe have studied the magneto-electroluminescence (MEL) response in light emitting diodes based on 2D-(PEA)PbI and 3D-MAPbI hybrid organic-inorganic perovskites at cryogenic temperatures. We found that the MEL is negative, i.e.
View Article and Find Full Text PDFTrans-polyacetylene [t-(CH)_{x}] possesses twofold ground state degeneracy. Using the Su-Schrieffer-Heeger Hamiltonian, scientists predicted charged solitons to be the primary photoexcitations in t-(CH)_{x}; this prediction, however, has led to sharp debate. To resolve this saga, we use subpicosecond transient photomodulation spectroscopy in the mid-IR spectral range (0.
View Article and Find Full Text PDFThe two-dimensional (2D) Ruddlesden-Popper organic-inorganic halide perovskites such as (2D)-phenethylammonium lead iodide (2D-PEPI) have layered structure that resembles multiple quantum wells (MQW). The heavy atoms in 2D-PEPI contribute a large spin-orbit coupling that influences the electronic band structure. Upon breaking the inversion symmetry, a spin splitting ('Rashba splitting') occurs in the electronic bands.
View Article and Find Full Text PDFNon-Hermitian Hamiltonians may still have real eigenvalues, provided that a combined parity-time (ƤƮ) symmetry exists. The prospect of ƤƮ symmetry has been explored in several physical systems such as photonics, acoustics, and electronics. The eigenvalues in these systems undergo a transition from real to complex at exceptional points (EPs), where the ƤƮ symmetry is broken.
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